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Moving to CC services
PSbosker, how much space is available on the drive that contains the operating system? Due to the collaborative nature of the feature, the synced files for Creative Cloud libraries are stored on the same purpose that contains the OS.
Ensure the drive containing the operating system has sufficient disk space for temporary files and any files you wish to use within Creative Cloud libraries.
You can also use the process in https://helpx.adobe.com/creative-cloud/help/import-export-creative-cloud-libraries.html to export and backup any libraries you have created but are no longer using.
You may also want to try signing out of your Adobe ID and back in again from within Photoshop directly under the Help menu.